All-Ambient Processed Binary CsPbBr3–CsPb2Br5 Perovskites with Synergistic Enhancement for High-Efficiency Cs–Pb–Br-Based Solar Cells

All-inorganic CsPbBr3 perovskite solar cells display outstanding stability toward moisture, light soaking, and thermal stressing, demonstrating great potential in tandem solar cells and toward commercialization. Unfortunately, it is still challenging to prepare high-performance CsPbBr3 films at moderate temperatures. Herein, a uniform, compact CsPbBr3 film was fabricated using its quantum dot (QD)-based ink precursor. The film was then treated using thiocyanate ethyl acetate (EA) solution in all-ambient conditions to produce a superior CsPbBr3-CsPb2Br5 composite film with a larger grain size and minimal defects. The achievement was attributed to the surface dissolution and recrystallization of the existing SCN- and EA. More specifically, the SCN- ions were first absorbed on the Pb atoms, leading to the dissolution and stripping of Cs+ and Br- ions from the CsPbBr3 QDs. On the other hand, the EA solution enhances the diffusion dynamics of surface atoms and the surfactant species. It is found that a small amount of CsPb2Br5 in the composite film gives the best surface passivation, while the Br-rich surface decreases Br vacancies (VBr) for a prolonged carrier lifetime. As a result, the fabricated device gives a higher solar cell efficiency of 6.81% with an outstanding long-term stability.